“2D-Materials LEGO” has a new component: Evidence for a single-layer van der Waals multiferroic

An international collaboration among the experimental groups led by Prof. Riccardo Comin and Prof. Nuh Gedik at Massachussets Institute of Technology and the theoretical groups led by Dr. Silvia Picozzi at CNR-SPIN and by Prof. Antia Botana at Arizona State University resulted in the discovery of multiferroicity persisting down to the monolayer limit.

Multiferroic materials have attracted wide interest because of their exceptional static  and dynamical  magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization through various mechanisms, the intrinsic coupling between the magnetic and dipolar order parameters resulting in high-strength magnetoelectric effects. Two-dimensional materials possessing such intrinsic multiferroic properties have been long sought for to enable the harnessing of magnetoelectric coupling in nanoelectronic devices. In their recent Nature paper , the authors report the discovery of type-II multiferroic order in a single atomic layer of the transition-metal-based van der Waals material NiI2. The multiferroic state of NiI2 is characterized by a proper-screw spin helix with given handedness, which couples to the charge degrees of freedom to produce a chirality-controlled electrical polarization. The authors use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Combining birefringence and second-harmonic-generation measurements with theoretical modelling and simulations, the authors detect a highly anisotropic electronic state that simultaneously breaks three-fold rotational and inversion symmetry, and supports polar order. The evolution of the optical signatures as a function of temperature and layer number surprisingly reveals an ordered magnetic polar state that persists down to the ultrathin limit of monolayer NiI2. These observations establish NiI2 and transition metal dihalides as a new platform for studying emergent multiferroic phenomena, chiral magnetic textures and ferroelectricity in the two-dimensional limit.

 

Song Q., Occhialini C.A., Ergecen E., Ilyas B., Amoroso D., Barone P., Kapeghian J., Watanabe K., Taniguchi T., Botana A. S., Picozzi S., Gedik N., Comin R.

Evidence for a single-layer van der Waals multiferroic

Nature 602, 601 (2022)

 

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